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Due to significant response contradictions, unidirectional carrier transmission of typical semiconductor p‐n junctions limits integrated sensors and artificial synapses in a monolithic device. In this work, a bipolar p‐n junction designed by employing the hydrogel/p‐GaN local contact interface with p‐GaN/(In,Ga)N heterojunction, demonstrating the bidirectional photocurrent and sensor/artificial synapse dual‐mode device successfully. After modifying Au nanoparticles, the negative (positive) photocurrent is increased by 900% (300%) under 365 nm (520 nm) light to achieve a more balanced bipolar carrier dynamic. Such a regulation of photocurrent is found to be attributed to the promotion of hydrogen evolution reaction (HER) at the hydrogel/Au/p‐GaN interface. Thus, the device achieves the ultrahigh paired‐pulse facilitation (PPF) index of 243% under self‐powered condition. Moreover, the implementation of plasticity from short‐term to long‐term demonstrates its adaptability in neural morphology visual recognition. Beyond independent working mode, the function of five classic logic gates is achieved under three‐terminal operation. Finally, an encrypted wireless communication system using dual‐channel light signals demonstrates the extensive application potential of the monolithic device. Therefore, this work presents a viable construction blueprint to meet the demands of next‐generation all‐in‐one optoelectronics for intricate application scenarios. [ABSTRACT FROM AUTHOR]

Cooperation of transition metal catalysis with photocatalysis is an emerging powerful approach to achieve coupling reactions for the synthesis of important chemicals. Owing to their facilely modulated structures and properties via reticular chemistry, photoactive covalent organic frameworks (COFs) arise quickly in building metallaphotocatalytic platforms targeting more efficient and sustainable protocol. In this Minireview, we summarize the recent advances in COFs‐based (integrated) platforms to forge carbon‐carbon/heteroatom (C, B, N, O, P, and S, etc.) bonds via a variety of cross‐coupling reactions driven by light, with focuses on the engineering of COFs' backbone, as well as the organization mode of COFs and metal site promoted catalytic performance. We also highlight the essential role of the underlying electron/energy processes in metallated COFs platforms (M@COFs). Aiming to guide catalysts' design to achieve more efficient performance or currently challenging transformations, we give our perspectives in this under‐developed yet promising field. [ABSTRACT FROM AUTHOR]